DNA Sequencing with Single-Stranded DNA Rectification in a Nanogap Gated by N‑Terminated Carbon Nanotube Electrodes
Само за регистроване кориснике
2020
Аутори
Đurišić, IvanaDražić, Miloš S.
Tomović, Aleksandar Ž.
Spasenović, Marko
Šljivančanin, Željko
Jovanović, Vladimir P.
Žikić, Radomir
Чланак у часопису (Објављена верзија)
,
© 2020 American Chemical Society
Метаподаци
Приказ свих података о документуАпстракт
Fast, reliable, and inexpensive DNA sequencing is an important pursuit in healthcare, especially in personalized medicine with possible deep societal impacts. Despite significant progress in various nanopore-based sequencing configurations, challenges that remain in resolution and chromosome-size-long readout call for new approaches. Here we found strong rectification in the transversal current during single-stranded DNA translocation through a nanopore with side-embedded N-terminated carbon nanotube electrodes. Employing density functional theory and nonequilibrium Green’s function formalisms, we show that the rectifying ratio (response to square pulses of alternating bias) bears high nucleobase specificity. Rectification arises because of bias-dependent resistance asymmetry on the deoxyribonucleotide−electrode interfaces. The asymmetry induces molecular charging and highest occupied molecular orbital pinning to the electrochemical potential of one of the electrodes, assisted by an in...-gap electric-field effect caused by dipoles at the terminated electrode ends. We propose the rectifying ratio, due to its order-of-magnitude-difference nucleobase selectivity and robustness to electrode-molecule orientation, as a promising readout quantifier for single-base resolution and chromosome-size-long single-read DNA sequencing. The proposed configurations are within experimental reach from the viewpoint of both nanofabrication and small current measurement.
Кључне речи:
nanogap / field effect / current rectification / local gating / DNA sequencing / density functional theory / nonequilibrium Green’s functionИзвор:
ACS Applied Nano Materials, 2020, 3, 3, 3034-3043Финансирање / пројекти:
- Електронске, транспортне и оптичке особине нанофазних материјала (RS-MESTD-Basic Research (BR or ON)-171033)
- Интегрална студија идентификације регионалних генетских фактора ризика и фактора ризика животне средине за масовне незаразне болести хумане популације у Србији - INGEMA_S (RS-MESTD-Integrated and Interdisciplinary Research (IIR or III)-41028)
- Swiss National Science Foundation (SCOPES Project 152406)
- NanoTools for Ultra Fast DNA Sequencing (EU-FP7-214840)
DOI: 10.1021/acsanm.0c00385
ISSN: 2574-0970
WoS: 000526396200097
Scopus: 2-s2.0-85088388401
Институција/група
VinčaTY - JOUR AU - Đurišić, Ivana AU - Dražić, Miloš S. AU - Tomović, Aleksandar Ž. AU - Spasenović, Marko AU - Šljivančanin, Željko AU - Jovanović, Vladimir P. AU - Žikić, Radomir PY - 2020 UR - https://vinar.vin.bg.ac.rs/handle/123456789/9097 AB - Fast, reliable, and inexpensive DNA sequencing is an important pursuit in healthcare, especially in personalized medicine with possible deep societal impacts. Despite significant progress in various nanopore-based sequencing configurations, challenges that remain in resolution and chromosome-size-long readout call for new approaches. Here we found strong rectification in the transversal current during single-stranded DNA translocation through a nanopore with side-embedded N-terminated carbon nanotube electrodes. Employing density functional theory and nonequilibrium Green’s function formalisms, we show that the rectifying ratio (response to square pulses of alternating bias) bears high nucleobase specificity. Rectification arises because of bias-dependent resistance asymmetry on the deoxyribonucleotide−electrode interfaces. The asymmetry induces molecular charging and highest occupied molecular orbital pinning to the electrochemical potential of one of the electrodes, assisted by an in-gap electric-field effect caused by dipoles at the terminated electrode ends. We propose the rectifying ratio, due to its order-of-magnitude-difference nucleobase selectivity and robustness to electrode-molecule orientation, as a promising readout quantifier for single-base resolution and chromosome-size-long single-read DNA sequencing. The proposed configurations are within experimental reach from the viewpoint of both nanofabrication and small current measurement. T2 - ACS Applied Nano Materials T1 - DNA Sequencing with Single-Stranded DNA Rectification in a Nanogap Gated by N‑Terminated Carbon Nanotube Electrodes VL - 3 IS - 3 SP - 3034 EP - 3043 DO - 10.1021/acsanm.0c00385 ER -
@article{ author = "Đurišić, Ivana and Dražić, Miloš S. and Tomović, Aleksandar Ž. and Spasenović, Marko and Šljivančanin, Željko and Jovanović, Vladimir P. and Žikić, Radomir", year = "2020", abstract = "Fast, reliable, and inexpensive DNA sequencing is an important pursuit in healthcare, especially in personalized medicine with possible deep societal impacts. Despite significant progress in various nanopore-based sequencing configurations, challenges that remain in resolution and chromosome-size-long readout call for new approaches. Here we found strong rectification in the transversal current during single-stranded DNA translocation through a nanopore with side-embedded N-terminated carbon nanotube electrodes. Employing density functional theory and nonequilibrium Green’s function formalisms, we show that the rectifying ratio (response to square pulses of alternating bias) bears high nucleobase specificity. Rectification arises because of bias-dependent resistance asymmetry on the deoxyribonucleotide−electrode interfaces. The asymmetry induces molecular charging and highest occupied molecular orbital pinning to the electrochemical potential of one of the electrodes, assisted by an in-gap electric-field effect caused by dipoles at the terminated electrode ends. We propose the rectifying ratio, due to its order-of-magnitude-difference nucleobase selectivity and robustness to electrode-molecule orientation, as a promising readout quantifier for single-base resolution and chromosome-size-long single-read DNA sequencing. The proposed configurations are within experimental reach from the viewpoint of both nanofabrication and small current measurement.", journal = "ACS Applied Nano Materials", title = "DNA Sequencing with Single-Stranded DNA Rectification in a Nanogap Gated by N‑Terminated Carbon Nanotube Electrodes", volume = "3", number = "3", pages = "3034-3043", doi = "10.1021/acsanm.0c00385" }
Đurišić, I., Dražić, M. S., Tomović, A. Ž., Spasenović, M., Šljivančanin, Ž., Jovanović, V. P.,& Žikić, R.. (2020). DNA Sequencing with Single-Stranded DNA Rectification in a Nanogap Gated by N‑Terminated Carbon Nanotube Electrodes. in ACS Applied Nano Materials, 3(3), 3034-3043. https://doi.org/10.1021/acsanm.0c00385
Đurišić I, Dražić MS, Tomović AŽ, Spasenović M, Šljivančanin Ž, Jovanović VP, Žikić R. DNA Sequencing with Single-Stranded DNA Rectification in a Nanogap Gated by N‑Terminated Carbon Nanotube Electrodes. in ACS Applied Nano Materials. 2020;3(3):3034-3043. doi:10.1021/acsanm.0c00385 .
Đurišić, Ivana, Dražić, Miloš S., Tomović, Aleksandar Ž., Spasenović, Marko, Šljivančanin, Željko, Jovanović, Vladimir P., Žikić, Radomir, "DNA Sequencing with Single-Stranded DNA Rectification in a Nanogap Gated by N‑Terminated Carbon Nanotube Electrodes" in ACS Applied Nano Materials, 3, no. 3 (2020):3034-3043, https://doi.org/10.1021/acsanm.0c00385 . .